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Distinct transient structural rearrangement of ionized water revealed by XFEL X-ray pump X-ray probe experiment

Title: Distinct transient structural rearrangement of ionized water revealed by XFEL X-ray pump X-ray probe experiment
Authors: Stransky, M.; Lane, T.; Gorel, A.; Boutet, S.; Schlichting, I.; Mancuso, A.; Jurek, Z.; Ziaja, B.
Source: arXiv
Publication Year: 2024
Collection: Max Planck Society: MPG.PuRe
Description: Using X-ray free electron laser (XFEL) radiation to conduct an X-ray pump X-ray probe experiment, we studied strongly ionized water as part of our ongoing work on radiation damage. After irradiance with a pump pulse with a nominal fluence of ~5×105 J/cm2, we observed for pump-probe delays of 75 fs and longer an unexpected structural rearrangement, exhibiting a characteristic length scale of ~9 Å. Simulations suggest that the experiment probes a superposition of ionized water in two distinct regimes. In the first, fluences expected at the X-ray focus create nearly completely ionized water, which as a result becomes effectively transparent to the probe. In the second regime, out of focus pump radiation produces O1+ and O2+ ions, which rearrange due to Coulombic repulsion over 10s of fs. Importantly, structural changes in the low fluence regime have implications for the design of two-pulse X-ray experiments that aim to study unperturbed liquid samples. Our simulations account for two key observations in the experimental data: the decrease in ambient water signal and an increase in low-angle X-ray scattering. They cannot, however, account for the experimentally observed 9 Å feature. A satisfactory account of this feature presents a new challenge for theory.
Document Type: article in journal/newspaper
File Description: application/pdf
Language: English
Availability: https://hdl.handle.net/21.11116/0000-000E-7455-0; https://hdl.handle.net/21.11116/0000-000E-7457-E
Rights: info:eu-repo/semantics/openAccess
Accession Number: edsbas.293E857F
Database: BASE